Enhancing the Output Performance of Triboelectric Nanogenerator Through Regulation of its Internal Nano‐Architecture

Abstract Triboelectric Nanogenerator (TENG) has proven highly effective in converting mechanical energy into electrical energy. Previous research on manipulating microstructure for performance enhancement primarily focused on the surface of TENGs. In this study, an innovative bottom–up strategic design to control the internal nano‐architecture for the enhanced output of TENG is proposed. This multiscale structural design strategy consists of defect chemistry (angstrom‐scale), surface modification (nano‐scale), and spatial regulation of nanoparticles (meso‐scale), which helps explore the optimal utilization of TENG's internal structure. After fine‐tuning the nano‐architecture, the output voltage is significantly increased. This optimized TENG serves as a robust platform for developing self‐powered systems, including self‐powered electrochemical chlorination systems for sterilization. Additionally, through the utilization of multiscale simulations (density functional theory, all‐atom molecular dynamics, and dissipative particle dynamics), the underlying mechanisms governing how the optimized nanoparticle–polymer interface and spatial arrangement of nanoparticles influence the storage and transfer of charges are comprehensively elucidated. This study not only demonstrates the effectiveness of manipulating internal nano‐architecture to enhance TENG performance for practical applications but also provides invaluable insights into structural engineering for TENG advancement.